Cr(VI), which has toxic effects, is a heavy metal and it must be removed from the environment due to the various damages it causes. In this study, the removal of Cr(VI) pollutants from aqueous solutions with Fe3O4-based materials using a batch adsorption technique was investigated. Magnetically modified graphene nanoplatelet (GNP)-based nanocomposites were prepared and their structures were characterized by FTIR, XRD, SEM, BET, and TGA techniques. The effects of various physicochemical parameters such as adsorbent dose, contact time, initial Cr(VI) solution concentration, pH, and the presence of coexisting ions (NaCl) on the adsorption process were investigated. Accordingly, the optimum conditions for Cr(VI) removal were determined. Nonlinear Langmuir, Freundlich, and Temkin isotherm models and pseudo-first-order, pseudo-second-order, and Bangham kinetic models were used to investigate the adsorption mechanism. The experimental data relatively fit the second-order kinetic model and the Freundlich isotherm model. The maximum adsorption capacities for pure Fe3O4 (Fe:GNP 1:0), Fe:GNP (2:1), and Fe:GNP (1:1) nanocomposite materials at 298 K and pH of approximately 5 were obtained as 12.71 mg/g, 27.03 mg/g, and 62.27 mg/g, respectively. This result showed that Cr(VI) removal increased as the amount of GNP in the composite material increased. Generally, the results confirmed that magnetically modified GNP-based adsorbents are functional and promising materials that can be used for the removal of pollutants such as Cr(VI) from aqueous media.